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DOI | 10.1073/pnas.1813647116 |
Pore condensation and freezing is responsible for ice formation below water saturation for porous particles | |
David, Robert O.1; Marcolli, Claudia1; Fahrni, Jonas2; Qiu, Yuqing3; Sirkin, Yamila A. Perez3; Molinero, Valeria3; Mahrt, Fabian1; Bruhwiler, Dominik2; Lohmann, Ulrike1; Kanji, Zamin A.1 | |
2019 | |
发表期刊 | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA |
ISSN | 0027-8424 |
出版年 | 2019 |
卷号 | 116期号:17页码:8184-8189 |
文章类型 | Article |
语种 | 英语 |
国家 | Switzerland; USA |
英文摘要 | Ice nucleation in the atmosphere influences cloud properties, altering precipitation and the radiative balance, ultimately regulating Earth's climate. An accepted ice nucleation pathway, known as deposition nucleation, assumes a direct transition of water from the vapor to the ice phase, without an intermediate liquid phase. However, studies have shown that nucleation occurs through a liquid phase in porous particles with narrow cracks or surface imperfections where the condensation of liquid below water saturation can occur, questioning the validity of deposition nucleation. We show that deposition nucleation cannot explain the strongly enhanced ice nucleation efficiency of porous compared with nonporous particles at temperatures below -40 degrees C and the absence of ice nucleation below water saturation at -35 degrees C. Using classical nucleation theory (CNT) and molecular dynamics simulations (MDS), we show that a network of closely spaced pores is necessary to overcome the barrier for macroscopic ice-crystal growth from narrow cylindrical pores. In the absence of pores, CNT predicts that the nucleation barrier is insurmountable, consistent with the absence of ice formation in MDS. Our results confirm that pore condensation and freezing (PCF), i.e., a mechanism of ice formation that proceeds via liquid water condensation in pores, is a dominant pathway for atmospheric ice nucleation below water saturation. We conclude that the ice nucleation activity of particles in the cirrus regime is determined by the porosity and wettability of pores. PCF represents a mechanism by which porous particles like dust could impact cloud radiative forcing and, thus, the climate via ice cloud formation. |
英文关键词 | ice nucleation clouds cirrus deposition nucleation pore condensation and freezing |
领域 | 地球科学 ; 气候变化 ; 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000465363700022 |
WOS关键词 | DEPOSITION NUCLEATION ; DUST ; IMMERSION ; SIZE ; ADSORPTION ; SORPTION ; NUCLEI ; PARAMETERIZATION ; CRYSTALLIZATION ; MECHANISMS |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/205095 |
专题 | 地球科学 资源环境科学 气候变化 |
作者单位 | 1.Swiss Fed Inst Technol, Dept Environm Syst Sci, Inst Atmospher & Climate Sci, CH-8092 Zurich, Switzerland; 2.Zurich Univ Appl Sci ZHAW, Inst Chem & Biotechnol, CH-8820 Wadenswil, Switzerland; 3.Univ Utah, Dept Chem, Salt Lake City, UT 84112 USA |
推荐引用方式 GB/T 7714 | David, Robert O.,Marcolli, Claudia,Fahrni, Jonas,et al. Pore condensation and freezing is responsible for ice formation below water saturation for porous particles[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2019,116(17):8184-8189. |
APA | David, Robert O..,Marcolli, Claudia.,Fahrni, Jonas.,Qiu, Yuqing.,Sirkin, Yamila A. Perez.,...&Kanji, Zamin A..(2019).Pore condensation and freezing is responsible for ice formation below water saturation for porous particles.PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,116(17),8184-8189. |
MLA | David, Robert O.,et al."Pore condensation and freezing is responsible for ice formation below water saturation for porous particles".PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA 116.17(2019):8184-8189. |
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